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The catalytic hydrodechlorination activity of bimetals can be well described by the volcano curve and rationally explained by the hydrogen adsorption energies on the metals, and was severely impaired by increasing Cr(VI) concentrations. Characterization results validated the formations of Fe(III)-Cr(III) hydroxide/oxyhydroxide on the bimetals surface after reacting with 4-CP and Cr(VI). This work provides the first insight into the catalytic properties of transition-metal modified nZVI for the effective removal of combined pollutants.A